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Organic Solvent-Free, One-Step Engineering of Graphene-Based Magnetic-Responsive Hybrids Using Design of Experiment-Driven Mechanochemistry.

ABSTRACT: In this study, we propose an organic solvent-free, one-step mechanochemistry approach to engineer water-dispersible graphene oxide/superparamagnetic iron oxide (GO/SPIOs) hybrids, for biomedical applications. Although mechanochemistry has been proposed in the graphene field for applications such as drug loading, exfoliation or polymer-composite formation, this is the first study to report mechanochemistry for preparation of GO/SPIOs hybrids. The statistical design of experiment (DoE) was employed to control the process parameters. DoE has been used to control formulation processes of other types of nanomaterials. The implementation of DoE for controlling the formulation processes of graphene-based nanomaterials is, however, novel. DoE approach could be of advantage as one can tailor GO-based hybrids of predicted yields and compositions. Hybrids were characterized by TEM, AFM FT-IR, Raman spectroscopy, and TGA. The dose-response magnetic resonance (MR) properties were confirmed by MR imaging of phantoms. The biocompatibility of the hybrids with A549 and J774 cell lines was confirmed by the modified LDH assay.

SUBMITTER: Mei KC

PROVIDER: S-EPMC4500448 | biostudies-literature | 2015 Jul

REPOSITORIES: biostudies-literature

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Organic Solvent-Free, One-Step Engineering of Graphene-Based Magnetic-Responsive Hybrids Using Design of Experiment-Driven Mechanochemistry.

Mei Kuo-Ching KC Guo Yukuang Y Bai Jie J Costa Pedro M PM Kafa Houmam H Protti Andrea A Hider Robert C RC Al-Jamal Khuloud T KT

ACS applied materials & interfaces 20150625 26

In this study, we propose an organic solvent-free, one-step mechanochemistry approach to engineer water-dispersible graphene oxide/superparamagnetic iron oxide (GO/SPIOs) hybrids, for biomedical applications. Although mechanochemistry has been proposed in the graphene field for applications such as drug loading, exfoliation or polymer-composite formation, this is the first study to report mechanochemistry for preparation of GO/SPIOs hybrids. The statistical design of experiment (DoE) was employe ...[more]

PMID: 26101940

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Project description:Inspired by Nature's tunability driven by the modulation of structural organization, we utilize peptide motifs as an approach to tailor not only hierarchical structure, but also thermo-responsive shape memory properties of conventional polymeric materials. Specifically, poly(β-benzyl-L-aspartate)-b-poly(dimethylsiloxane)-b-poly(β-benzyl-L-aspartate) was incorporated as the soft segment in peptide-polyurea hybrids to manipulate hierarchical ordering through peptide secondary structure and a balance of inter- and intra-molecular hydrogen bonding. Employing these bioinspired peptidic polyureas, we investigated the influence of secondary structure on microphase-separated morphology, and shape fixity and recovery via attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR), small-angle X-ray scattering (SAXS) and dynamic mechanical analysis (DMA). The β-sheet motifs promoted phase mixing through extensive inter-molecular hydrogen bonding between the hard block and peptide segments and provided an increased chain elasticity, resulting in decreased shape fixity compared to a non-peptidic control. In contrast, intra-molecular hydrogen bonding driven by the α-helical arrangements yielded a microphase-separated and hierarchically ordered morphology, leading to an increase in the shape fixing ratio. These results indicate that peptide secondary structure provides a convenient handle for tuning shape memory properties by regulating hydrogen bonding with the surrounding polyurea hard segment, wherein extent of hydrogen bonding and phase mixing between the peptidic block and hard segment dictate the resulting shape memory behaviour. Furthermore, the ability to shift secondary structure as a function of temperature was also demonstrated as a pathway to influence shape memory response. This research highlights that peptide secondary conformation influences the hierarchical ordering and modulates the shape memory response of peptide-polymer hybrids. We anticipate that these findings will enable the design of smart bio-inspired materials with responsive and tailored function via a balance of hydrogen bonding character, structural organization, and mechanics.

Dataset Information

Organic Solvent-Free, One-Step Engineering of Graphene-Based Magnetic-Responsive Hybrids Using Design of Experiment-Driven Mechanochemistry.

Publications

Organic Solvent-Free, One-Step Engineering of Graphene-Based Magnetic-Responsive Hybrids Using Design of Experiment-Driven Mechanochemistry.

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